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Stewart J Clark

Publications and source records attributed to Stewart J Clark.

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Re-evaluating photoluminescent defects in Cu$_2$O

Defects in cuprous oxide (Cu$_2$O) strongly influence its performance in applications ranging from photovoltaics to emerging quantum technologies based on Rydberg excitons where microscopic crystal purity is essential. Photoluminescence (PL) spectroscopy is widely used as a diagnostic of material quality yet the origins of the sub-band-gap PL lines remain controversial despite decades of study. Using density functional theory we systematically evaluate native point defects in Cu$_2$O and identify which produce robust electronic states within the band gap. By combining supercell-size convergence criteria and cross-functional consistency checks we show that the widely accepted assignments of the 1.35\,eV, 1.5\,eV, and 1.7\,eV PL lines to copper and oxygen vacancies are unsupported. Instead we find that oxygen interstitials, copper interstitials and one form of split copper vacancy are the only native defects that consistently introduce true in-gap states. These results provide a revised framework for interpreting PL spectra and offer a more reliable basis for diagnosing crystal quality in Cu$_2$O-based quantum-device platforms.

cond-mat.mtrl-sci

Microwave-optical spectroscopy of Rydberg excitons in the ultrastrong driving regime

We study the ultrastrong driving of Rydberg excitons in Cu$_2$O by a microwave field. The effect of the field is studied using optical absorption spectroscopy, and through the observation of sidebands on the transmitted laser light. A model based on Floquet theory is constructed to study the system beyond the rotating wave approximation. We obtain near quantitative agreement between theory and experiment across a 16-fold range of microwave field strengths spanning from the perturbative to the ultrastrong driving regime. Compared to Rydberg atoms, the large non-radiative widths of Rydberg excitons leads to new behaviour such as the emergence of an absorption continuum without ionization.

cond-mat.mes-hall